The Coalescence Behavior of Two-Dimensional Materials Revealed by Multiscale Imaging during Chemical Vapor Deposition Growth.

Wafer-scale monocrystalline two-dimensional (2D) materials can theoretically be grown by seamless coalescence of individual domains into a large single crystal. Here we present a concise study of the coalescence behavior of crystalline 2D films using a combination of complementary methods. Direct observation of overlayer growth from the atomic to the millimeter scale and under model- and industrially relevant growth conditions reveals the influence of the film-substrate interaction on the crystallinity of the 2D film.

In situ observations of an active MoS model hydrodesulfurization catalyst.

The hydrodesulfurization process is one of the cornerstones of the chemical industry, removing harmful sulfur from oil to produce clean hydrocarbons. The reaction is catalyzed by the edges of MoS nanoislands and is operated in hydrogen-oil mixtures at 5-160 bar and 260-380 °C. Until now, it has remained unclear how these harsh conditions affect the structure of the catalyst.

On the Non-trivial Origin of Atomic-Scale Patterns in Friction Force Microscopy.

Friction between two surfaces is due to nano- and micro-asperities at the interface that establish true contact and are responsible for the energy dissipation. To understand the friction mechanism, often single-asperity model experiments are conducted in atomic-force microscopes. Here, we show that the conventional interpretation of the typical results of such experiments, based on a simple mass-spring model, hides a fundamental contradiction.

Structural Dynamics of AlO/NiAl(110) During Film Growth in NO.

While continuum descriptions of oxide film growth are well established, the local structural dynamics during oxide growth are largely unexplored. Here, we investigate this using scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS) for the example of alumina film growth on NiAl(110) following NO exposure. To maintain a well-defined system, we have adopted a cyclic growth approach of NO adsorption and annealing.

Observing the oxidation of platinum.

Despite its importance in oxidation catalysis, the active phase of Pt remains uncertain, even for the Pt(111) single-crystal surface. Here, using a ReactorSTM, the catalytically relevant structures are identified as two surface oxides, different from bulk α-PtO, previously observed. They are constructed from expanded oxide rows with a lattice constant close to that of α-PtO, either assembling into spoked wheels, 1-5 bar O, or closely packed in parallel lines, above 2.

Simultaneous scanning tunneling microscopy and synchrotron X-ray measurements in a gas environment.

A combined X-ray and scanning tunneling microscopy (STM) instrument is presented that enables the local detection of X-ray absorption on surfaces in a gas environment. To suppress the collection of ion currents generated in the gas phase, coaxially shielded STM tips were used. The conductive outer shield of the coaxial tips can be biased to deflect ions away from the tip core.

In Situ Optical Reflectance Difference Observations of CO Oxidation over Pd(100).

Using a home-built reflectometer, we have investigated the changes in the optical reflectivity of a Pd(100) model catalyst during CO oxidation under high-pressure, high-temperature conditions. We observe changes in optical contrast when exposing the surface to CO oxidation conditions at 200 mbar from room temperature up to 400 °C. These changes in reflectivity are a result both of the formation of a surface oxide layer and of a change in surface roughness because of gas exposure.

Surface science under reaction conditions: CO oxidation on Pt and Pd model catalysts.

Platinum and palladium are frequently used as catalytic materials, for example for the oxidation of CO. This is one of the most widely studied reactions in the field of surface science. Although seemingly uncomplicated, it remains an active and interesting topic, which is partially explained by the push to conduct experiments on model systems under relevant reaction conditions.

From dull to shiny: A novel setup for reflectance difference analysis under catalytic conditions.

We have developed an experimental setup for optically monitoring a catalytically active surface under reaction conditions. A flow reactor with optical access allows us to image the behavior of an active catalyst surface down to the millimeter length scale. We use reflectance difference measurements with 625 nm light to investigate CO oxidation on Pd(100) at 300 mbar and 320 °C.

In situ TEM observation of the Boudouard reaction: multi-layered graphene formation from CO on cobalt nanoparticles at atmospheric pressure.

Using a MEMS nanoreactor in combination with a specially designed in situ Transmission Electron Microscope (TEM) holder and gas supply system, we imaged the formation of multiple layers of graphene encapsulating a cobalt nanoparticle, at 1 bar CO : N (1 : 1) and 500 °C. The cobalt nanoparticle was imaged live in a TEM during the Boudouard reaction. The in situ/operando TEM studies give insight into the behaviour of the catalyst at the nanometer-scale, under industrially relevant conditions.

Combined scanning probe microscopy and x-ray scattering instrument for in situ catalysis investigations.

We have developed a new instrument combining a scanning probe microscope (SPM) and an X-ray scattering platform for ambient-pressure catalysis studies. The two instruments are integrated with a flow reactor and an ultra-high vacuum system that can be mounted easily on the diffractometer at a synchrotron end station. This makes it possible to perform SPM and X-ray scattering experiments in the same instrument under identical conditions that are relevant for catalysis.

In situ observation of self-assembled hydrocarbon Fischer-Tropsch products on a cobalt catalyst.

Fischer-Tropsch synthesis is a heterogeneous catalytic reaction that creates approximately 2% of the world's fuel. It involves the synthesis of linear hydrocarbon molecules from a gaseous mixture of carbon monoxide and hydrogen at high pressures (from a few to tens of bars) and high temperatures (200-350 °C). To gain further insight into the fundamental mechanisms of this industrial process, we have used a purpose-built scanning tunnelling microscope to monitor a cobalt model catalyst under reaction conditions.

Shape and Size of Cobalt Nanoislands Formed Spontaneously on Cobalt Terraces during Fischer-Tropsch Synthesis.

Cobalt-based catalysts undergo a massive and spontaneous reconstruction to form uniform triangular nanoislands under Fischer-Tropsch (FT) conditions. This reconstruction is driven by the unusual and synergistic adsorption of square-planar carbon and CO at the 4-fold edge sites of the nanoislands, driving the formation of triangular islands. The size of the nanoislands is determined by the balance between energy gain from creating C/CO-covered edges and energy penalty to create C/CO-covered corners.

Kinetics of graphene formation on Rh(111) investigated by in situ scanning tunneling microscopy.

In situ scanning tunneling microscopy observations of graphene formation on Rh(111) show that the moiré pattern between the lattices of the overlayer and substrate has a decisive influence on the growth. The process is modulated in the large unit cells of the moiré pattern. We distinguish two steps: the addition of a unit cell that introduces one or more new kinks and the addition of further unit cells that merely advance the position of an existing kink.

Reversible formation of a PdC(x) phase in Pd nanoparticles upon CO and O2 exposure.

The structure and chemical composition of Pd nanoparticles exposed to pure CO and mixtures of CO and O(2) at elevated temperatures have been studied in situ by a combination of X-ray Diffraction and X-ray Photoelectron Spectroscopy in pressures ranging from ultra high vacuum to 10 mbar and from room temperature to a few hundred degrees celsius. Our investigation shows that under CO exposure, above a certain temperature, carbon dissolves into the Pd particles forming a carbide phase. Upon exposure to CO and O(2) mixtures, the carbide phase forms and disappears reversibly, switching at the stoichiometric ratio for CO oxidation.

A general model of metal underpotential deposition in the presence of thiol-based additives based on an in situ STM study.

Bis(3-sulfopropyl)disulfide (SPS) is a common additive in commercial copper electroplating baths. We have studied the influence of SPS on Cu underpotential deposition (UPD) on a Au(111) single crystal surface by means of cyclic voltammetry (CV) and electrochemical scanning tunneling microscopy (EC-STM). By combining our results with the results from the literature we propose a model that describes different stages of Cu UPD in the presence of SPS.

The role of steps in surface catalysis and reaction oscillations.

Atomic steps at the surface of a catalyst play an important role in heterogeneous catalysis, for example as special sites with increased catalytic activity. Exposure to reactants can cause entirely new structures to form at the catalyst surface, and these may dramatically influence the reaction by 'poisoning' it or by acting as the catalytically active phase. For example, thin metal oxide films have been identified as highly active structures that form spontaneously on metal surfaces during the catalytic oxidation of carbon monoxide.

How boron nitride forms a regular nanomesh on Rh(111).

Boron nitride forms nearly perfectly regular films with a thickness of precisely one atom on various metal surfaces. Here, we follow the formation of boron nitride layers on Rh(111) with scanning tunneling microscopy (STM) under realistic growth conditions, up to 1200 K. Our STM movies demonstrate in detail how the structure grows and how defects are introduced.

The description of friction of silicon MEMS with surface roughness: virtues and limitations of a stochastic Prandtl-Tomlinson model and the simulation of vibration-induced friction reduction.

We have replaced the periodic Prandtl-Tomlinson model with an atomic-scale friction model with a random roughness term describing the surface roughness of micro-electromechanical systems (MEMS) devices with sliding surfaces. This new model is shown to exhibit the same features as previously reported experimental MEMS friction loop data. The correlation function of the surface roughness is shown to play a critical role in the modelling.

Torque and twist against superlubricity.

Superlubricity between incommensurate surfaces provides a desired low-friction state essential for the function of small-scale machines. Here we demonstrate experimentally and theoretically that superlubricity in contacts lubricated by lamellar solids might be eliminated due to torque-induced reorientation coupled to lateral motion. We find that the possibility of reorientation always leads to stabilization of a high frictional state which corresponds to a commensurate configuration.

Superlubricity of graphite.

Using a home-built frictional force microscope that is able to detect forces in three dimensions with a lateral force resolution down to 15 pN, we have studied the energy dissipation between a tungsten tip sliding over a graphite surface in dry contact. By measuring atomic-scale friction as a function of the rotational angle between two contacting bodies, we show that the origin of the ultralow friction of graphite lies in the incommensurability between rotated graphite layers, an effect proposed under the name of "superlubricity" [Phys. Rev.

The ring structure and organization of light harvesting 2 complexes in a reconstituted lipid bilayer, resolved by atomic force microscopy.

The main function of the transmembrane light-harvesting complexes in photosynthetic organisms is the absorption of a light quantum and its subsequent rapid transfer to a reaction center where a charge separation occurs. A combination of freeze-thaw and dialysis methods were used to reconstitute the detergent-solubilized Light Harvesting 2 complex (LH2) of the purple bacterium Rhodopseudomonas acidophila strain 10050 into preformed egg phosphatidylcholine liposomes, without the need for extra chemical agents. The LH2-containing liposomes opened up to a flat bilayer, which were imaged with tapping and contact mode atomic force microscopy under ambient and physiological conditions, respectively.